Journal
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
Volume 141, Issue 50, Pages 19888-19901Publisher
AMER CHEMICAL SOC
DOI: 10.1021/jacs.9b11195
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Funding
- National Natural Science Foundation of China (NSFC) [21761132022]
- DFG [391643887, GL307/4-1, C0802/2, C0802/4-1]
- Cluster of Excellence Macromolecular Complexes Frankfurt
- NSFC [21922301, 21673074]
- Ministry of Science and Technology of China [2016YFA0501700]
- Shanghai Municipal Natural Science Foundation [18ZR1412600]
- youth topnotch talent support program of Shanghai
- NYUECNU Center for Computational Chemistry at NYU Shanghai
- Goethe University of Frankfurt am Main via FOKUS program
- [DEG/SFB807]
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Although the rapid development of sensitivity-enhanced solid-state NMR (ssNMR) spectroscopy based on dynamic nuclear polarization (DNP) has enabled a broad range of novel applications in material and life sciences, further methodological improvements are needed to unleash the full potential of DNP-ssNMR. Here, a new methyl-based toolkit for exploring protein structures is presented, which combines signal-enhancement by DNP with heteronuclear Overhauser effect (hetNOE), carbon-carbon-spin diffusion (SD) and strategically designed isotope-labeling schemes. It is demonstrated that within this framework, methyl groups can serve as dynamic sensors for probing local molecular packing within proteins. Furthermore, they can be used as NMR torches to selectively enlighten their molecular environment, e.g., to selectively enhance the polarization of nuclei within residues of ligand-binding pockets. Finally, the use of C-13-C-13 spin diffusion enables probing carbon-carbon distances within the subnanometer range, which bridges the gap between conventional C-13-ssNMR methods and EPR spectroscopy. The applicability of these methods is directly shown on a large membrane protein, the light-driven proton pump green proteorhodopsin (GPR), which offers new insight into the functional mechanism of the early step of its photocycle.
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